CN111135820A - Preparation method of barium-containing flue gas denitration catalyst and prepared denitration catalyst - Google Patents
Preparation method of barium-containing flue gas denitration catalyst and prepared denitration catalyst Download PDFInfo
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- CN111135820A CN111135820A CN201911393920.3A CN201911393920A CN111135820A CN 111135820 A CN111135820 A CN 111135820A CN 201911393920 A CN201911393920 A CN 201911393920A CN 111135820 A CN111135820 A CN 111135820A
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- barium
- denitration catalyst
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- 239000003054 catalyst Substances 0.000 title claims abstract description 55
- 229910052788 barium Inorganic materials 0.000 title claims abstract description 41
- DSAJWYNOEDNPEQ-UHFFFAOYSA-N barium atom Chemical compound [Ba] DSAJWYNOEDNPEQ-UHFFFAOYSA-N 0.000 title claims abstract description 41
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 title claims abstract description 20
- 239000003546 flue gas Substances 0.000 title claims abstract description 20
- 238000002360 preparation method Methods 0.000 title claims abstract description 10
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims abstract description 38
- 150000001553 barium compounds Chemical class 0.000 claims abstract description 21
- 239000000243 solution Substances 0.000 claims abstract description 19
- MUBZPKHOEPUJKR-UHFFFAOYSA-N Oxalic acid Chemical compound OC(=O)C(O)=O MUBZPKHOEPUJKR-UHFFFAOYSA-N 0.000 claims abstract description 18
- 239000004408 titanium dioxide Substances 0.000 claims abstract description 18
- 239000002994 raw material Substances 0.000 claims abstract description 15
- 239000000203 mixture Substances 0.000 claims abstract description 14
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 13
- 239000011259 mixed solution Substances 0.000 claims abstract description 12
- 239000000843 powder Substances 0.000 claims abstract description 11
- 238000001354 calcination Methods 0.000 claims abstract description 10
- 239000007864 aqueous solution Substances 0.000 claims abstract description 8
- QGZKDVFQNNGYKY-UHFFFAOYSA-O Ammonium Chemical compound [NH4+] QGZKDVFQNNGYKY-UHFFFAOYSA-O 0.000 claims abstract description 6
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims abstract description 6
- 229910052782 aluminium Inorganic materials 0.000 claims abstract description 6
- UNTBPXHCXVWYOI-UHFFFAOYSA-O azanium;oxido(dioxo)vanadium Chemical compound [NH4+].[O-][V](=O)=O UNTBPXHCXVWYOI-UHFFFAOYSA-O 0.000 claims abstract description 6
- 238000001035 drying Methods 0.000 claims abstract description 6
- 235000006408 oxalic acid Nutrition 0.000 claims abstract description 6
- 239000011230 binding agent Substances 0.000 claims abstract description 5
- 238000000465 moulding Methods 0.000 claims abstract 2
- 238000002525 ultrasonication Methods 0.000 claims abstract 2
- QVQLCTNNEUAWMS-UHFFFAOYSA-N barium oxide Chemical compound [Ba]=O QVQLCTNNEUAWMS-UHFFFAOYSA-N 0.000 claims description 16
- 238000000034 method Methods 0.000 claims description 15
- PEDCQBHIVMGVHV-UHFFFAOYSA-N Glycerine Chemical compound OCC(O)CO PEDCQBHIVMGVHV-UHFFFAOYSA-N 0.000 claims description 12
- 238000003756 stirring Methods 0.000 claims description 10
- RQPZNWPYLFFXCP-UHFFFAOYSA-L barium dihydroxide Chemical compound [OH-].[OH-].[Ba+2] RQPZNWPYLFFXCP-UHFFFAOYSA-L 0.000 claims description 8
- 229910001863 barium hydroxide Inorganic materials 0.000 claims description 8
- HZAXFHJVJLSVMW-UHFFFAOYSA-N 2-Aminoethan-1-ol Chemical compound NCCO HZAXFHJVJLSVMW-UHFFFAOYSA-N 0.000 claims description 6
- KXGFMDJXCMQABM-UHFFFAOYSA-N 2-methoxy-6-methylphenol Chemical group [CH]OC1=CC=CC([CH])=C1O KXGFMDJXCMQABM-UHFFFAOYSA-N 0.000 claims description 5
- 239000007788 liquid Substances 0.000 claims description 5
- 239000005011 phenolic resin Substances 0.000 claims description 5
- 229920001568 phenolic resin Polymers 0.000 claims description 5
- 239000004372 Polyvinyl alcohol Substances 0.000 claims description 2
- 229920002401 polyacrylamide Polymers 0.000 claims description 2
- 229920002451 polyvinyl alcohol Polymers 0.000 claims description 2
- 238000009736 wetting Methods 0.000 claims description 2
- 238000001125 extrusion Methods 0.000 abstract description 8
- 230000006835 compression Effects 0.000 abstract description 4
- 238000007906 compression Methods 0.000 abstract description 4
- 229920002521 macromolecule Polymers 0.000 abstract description 4
- 150000001875 compounds Chemical class 0.000 abstract description 2
- 230000009286 beneficial effect Effects 0.000 abstract 1
- GNTDGMZSJNCJKK-UHFFFAOYSA-N divanadium pentaoxide Chemical compound O=[V](=O)O[V](=O)=O GNTDGMZSJNCJKK-UHFFFAOYSA-N 0.000 description 8
- ZNOKGRXACCSDPY-UHFFFAOYSA-N tungsten trioxide Chemical compound O=[W](=O)=O ZNOKGRXACCSDPY-UHFFFAOYSA-N 0.000 description 8
- 239000003245 coal Substances 0.000 description 5
- 238000009210 therapy by ultrasound Methods 0.000 description 4
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 description 3
- MWUXSHHQAYIFBG-UHFFFAOYSA-N Nitric oxide Chemical compound O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 3
- 235000011114 ammonium hydroxide Nutrition 0.000 description 3
- 239000002131 composite material Substances 0.000 description 3
- 230000007547 defect Effects 0.000 description 3
- 238000005299 abrasion Methods 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 229920000742 Cotton Polymers 0.000 description 1
- 235000021355 Stearic acid Nutrition 0.000 description 1
- 229920006231 aramid fiber Polymers 0.000 description 1
- 239000012752 auxiliary agent Substances 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 238000010531 catalytic reduction reaction Methods 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 239000000428 dust Substances 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- QIQXTHQIDYTFRH-UHFFFAOYSA-N octadecanoic acid Chemical compound CCCCCCCCCCCCCCCCCC(O)=O QIQXTHQIDYTFRH-UHFFFAOYSA-N 0.000 description 1
- OQCDKBAXFALNLD-UHFFFAOYSA-N octadecanoic acid Natural products CCCCCCCC(C)CCCCCCCCC(O)=O OQCDKBAXFALNLD-UHFFFAOYSA-N 0.000 description 1
- 238000006722 reduction reaction Methods 0.000 description 1
- 239000008117 stearic acid Substances 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
Classifications
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/16—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
- B01J23/24—Chromium, molybdenum or tungsten
- B01J23/30—Tungsten
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
- B01D53/8621—Removing nitrogen compounds
- B01D53/8625—Nitrogen oxides
- B01D53/8628—Processes characterised by a specific catalyst
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/002—Mixed oxides other than spinels, e.g. perovskite
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/02—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the alkali- or alkaline earth metals or beryllium
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2258/00—Sources of waste gases
- B01D2258/02—Other waste gases
- B01D2258/0283—Flue gases
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2523/00—Constitutive chemical elements of heterogeneous catalysts
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Organic Chemistry (AREA)
- Environmental & Geological Engineering (AREA)
- Health & Medical Sciences (AREA)
- Biomedical Technology (AREA)
- Analytical Chemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Catalysts (AREA)
- Exhaust Gas Treatment By Means Of Catalyst (AREA)
Abstract
本发明公开一种含钡烟气脱硝催化剂的制备方法，涉及脱硝催化剂技术领域，包括以下步骤：(1)将偏钨酸铵和偏钒酸铵加入草酸溶液中，制得混合液；(2)往步骤(1)的混合液中加入钡化合物和二氧化钛水溶液，超声后，获得原料液；(3)将原料液置于100℃下干燥至恒重，煅烧；(4)加水润湿含钡催化剂粉末，添加铝水溶胶，加入有机粘接剂和成型助剂，调节混合物水分含量为15‑35％，挤出成型，制得含钡脱硝催化剂。本发明的有益效果在于：含钡化合物与二氧化钛大分子在450‑650℃之间煅烧的时候会发生晶格掺杂的现象，改变载体的抗压和耐磨性能。同时保障脱硝催化剂在300～400℃的温度范围内，脱硝效率达到95％以上。The invention discloses a preparation method of a barium-containing flue gas denitration catalyst, which relates to the technical field of denitration catalysts and includes the following steps: (1) adding ammonium metatungstate and ammonium metavanadate into an oxalic acid solution to prepare a mixed solution; (2) ) adding a barium compound and an aqueous solution of titanium dioxide to the mixed solution of step (1), and after ultrasonication, a raw material solution is obtained; (3) placing the raw material solution at 100° C., drying to constant weight, and calcining; (4) adding water to wet the barium-containing solution Catalyst powder, adding aluminum hydrosol, adding organic binder and molding aid, adjusting the moisture content of the mixture to 15-35%, and extrusion molding to prepare a barium-containing denitration catalyst. The beneficial effect of the invention is that: when the barium-containing compound and the titania macromolecules are calcined between 450-650° C., the phenomenon of lattice doping occurs, which changes the compression resistance and wear resistance of the carrier. At the same time, it is ensured that the denitration catalyst can achieve a denitration efficiency of more than 95% in the temperature range of 300-400 °C.
Description
Technical Field
The invention relates to the technical field of denitration catalysts, and particularly relates to a preparation method of a barium-containing flue gas denitration catalyst and the prepared denitration catalyst.
Background
The energy structure of China is mainly coal, the emission of NOx generated by the coal is increased year by year, and the coal is the first in the world at present.
At present, flue gas denitration is one of effective methods for controlling nitrogen oxide emission in a coal burning process, wherein a Selective Catalytic Reduction (SCR) technology is widely applied to flue gas denitration processes of coal burning power plants and non-electric power industries due to high denitration efficiency, good selectivity and stable and reliable operation. For example, patent CN101829560 discloses a denitration catalyst, which is composed of the following components in parts by weight: 70-90 parts of titanium dioxide, 8-15 parts of tungsten trioxide, 1.5-3 parts of vanadium pentoxide, 2-6 parts of aramid fiber, 3-6 parts of pulp cotton and 1.5-3 parts of stearic acid.
The catalyst is the core of the SCR technology, and the research on the catalytic material is always the research hotspot of the SCR technology. The existing SCR catalyst used in China at present can cause obvious reduction of denitration efficiency due to abrasion of the catalyst, the mechanical life decay is accelerated, and the catalyst needs to be replaced regularly. The denitration reactor is arranged between the economizer and the air preheater and is positioned in a high-temperature high-dust area, which means that the problems of uneven denitration flow field, abrasion and the like always exist.
Disclosure of Invention
The invention provides a barium-containing flue gas denitration catalyst, which aims to solve the technical problem that the existing denitration catalyst is easy to wear.
The invention solves the technical problems through the following technical means:
a preparation method of a barium-containing flue gas denitration catalyst comprises the following steps:
(1) adding 1-10 parts of ammonium metatungstate and 1-5 parts of ammonium metavanadate into an oxalic acid solution with the mass fraction of 2%, and stirring to obtain a mixed solution;
(2) adding a barium compound and a titanium dioxide aqueous solution into the mixed solution obtained in the step (1), and performing ultrasonic treatment to obtain a raw material solution; the barium compound is barium hydroxide or barium oxide;
(3) drying the raw material liquid at 100 ℃ to constant weight, and calcining to obtain barium-containing catalyst powder;
(4) wetting barium-containing catalyst powder with water, adding aluminum hydrosol, adding an organic binder and a forming auxiliary agent, stirring to obtain a mixture, adjusting the water content of the mixture to be 15-35%, and performing extrusion forming to obtain the barium-containing denitration catalyst.
Has the advantages that: the catalyst prepared by the invention takes the barium compound and the titanium dioxide as the composite carrier, the main active components are vanadium pentoxide and tungsten trioxide, and because the titanium dioxide has a large number of lattice defects, the barium-containing compound and titanium dioxide macromolecules can generate a lattice doping phenomenon when being calcined at the temperature of 450-650 ℃, so that the compression resistance and the wear resistance of the carrier are changed. Meanwhile, the denitration efficiency of the denitration catalyst can reach more than 95% within the temperature range of 300-400 ℃.
When the barium compound is barium hydroxide or barium oxide, the barium compound can replace ammonia water to be used, and the safety level of raw materials is reduced.
Preferably, the mass ratio of the barium compound to the titanium dioxide aqueous solution is 1: 4.
Preferably, the ultrasonic power in the step (2) is 300w, and the ultrasonic time is 1 h.
Preferably, the organic binder is phenolic resin, polyvinyl alcohol or polyacrylamide.
Preferably, the forming aid is glycerol or ethanolamine.
Preferably, the calcining temperature in the step (3) is 400-650 ℃, and the calcining time is 2-20 h.
Preferably, the purity of the barium compound is 95% or more.
The second technical problem to be solved by the present invention is to provide a barium-containing flue gas denitration catalyst prepared by the above preparation method.
The invention solves the technical problems through the following technical means:
a barium-containing flue gas denitration catalyst prepared by the preparation method.
Has the advantages that: the catalyst prepared by the invention takes the barium compound and the titanium dioxide as the composite carrier, the main active components are vanadium pentoxide and tungsten trioxide, and because the titanium dioxide has a large number of lattice defects, the phenomenon of lattice doping can occur when barium-containing micromolecules and titanium dioxide macromolecules are calcined at the temperature of 450-650 ℃, so that the compression resistance and the wear resistance of the carrier are changed. Meanwhile, the denitration efficiency of the denitration catalyst can reach more than 95% within the temperature range of 300-400 ℃.
When the barium compound is barium hydroxide or barium oxide, the barium compound can replace ammonia water to be used, and the safety level of raw materials is reduced.
The invention has the advantages that: the catalyst prepared by the invention takes the barium compound and the titanium dioxide as the composite carrier, the main active components are vanadium pentoxide and tungsten trioxide, and because the titanium dioxide has a large number of lattice defects, the phenomenon of lattice doping can occur when barium-containing micromolecules and titanium dioxide macromolecules are calcined at the temperature of 450-650 ℃, so that the compression resistance and the wear resistance of the carrier are changed. Meanwhile, the denitration efficiency of the denitration catalyst can reach more than 95% within the temperature range of 300-400 ℃.
When the barium compound is barium hydroxide or barium oxide, the barium compound can replace ammonia water to be used, and the safety level of raw materials is reduced.
Detailed Description
In order to make the objects, technical solutions and advantages of the embodiments of the present invention clearer, the technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the embodiments of the present invention, and it is obvious that the described embodiments are some embodiments of the present invention, but not all embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
Test materials, reagents and the like used in the following examples are commercially available unless otherwise specified.
The specific techniques or conditions not specified in the examples can be performed according to the techniques or conditions described in the literature in the field or according to the product specification.
Example 1
The preparation method of the barium-containing flue gas denitration catalyst comprises the following steps:
(1) adding 1 part of ammonium metatungstate and 1 part of ammonium metavanadate into 8 parts of oxalic acid solution with the mass fraction of 2%, stirring and mixing the mixed solution;
(2) adding 1 part of barium hydroxide and 4 parts of titanium dioxide aqueous solution into 1 part of the mixed solution obtained in the step (1), and carrying out ultrasonic treatment for 1 hour at the power of 300w to obtain a raw material solution; the barium compound in this example is barium hydroxide;
(3) drying the raw material liquid at 100 ℃ to constant weight, and calcining at 400 ℃ for 20h to prepare barium-containing catalyst powder;
(4) adding 1 part of water to wet 9 parts of barium-containing catalyst powder, adding 4 parts of aluminum hydrosol, adding 3 parts of phenolic resin and 2 parts of glycerol, stirring to obtain a mixture, adjusting the water content of the mixture to be 15%, and extruding the mixture into a honeycomb wet body by a double-screw extrusion method to obtain the barium-containing denitration catalyst; wherein the double screw extrusion method and the water content adjusting method are the prior art.
Example 2
(1) Adding 5 parts of ammonium metatungstate and 2 parts of ammonium metavanadate into 10 parts of oxalic acid solution with the mass fraction of 2%, and stirring to obtain a mixed solution;
(2) adding 2 parts of barium hydroxide and 8 parts of titanium dioxide aqueous solution into 3 parts of the mixed solution obtained in the step (1), and carrying out ultrasonic treatment for 1 hour under the power of 300w to obtain a raw material solution; the barium compound in this example is barium oxide;
(3) drying the raw material liquid at 100 ℃ to constant weight, and calcining at 500 ℃ for 10h to prepare barium-containing catalyst powder;
(4) adding 2 parts of water to wet 8 parts of barium-containing catalyst powder, adding 3 parts of aluminum hydrosol, adding 2 parts of phenolic resin and 3 parts of glycerol, stirring to obtain a mixture, adjusting the water content of the mixture to be 20%, and extruding the mixture into a honeycomb-shaped wet body by a double-screw extrusion method to obtain the barium-containing denitration catalyst; wherein the double screw extrusion method and the water content adjusting method are the prior art.
Example 3
(1) Adding 10 parts of ammonium metatungstate and 2 parts of ammonium metavanadate into 15 parts of oxalic acid solution with the mass fraction of 2%, and stirring to obtain a mixed solution;
(2) adding 2 parts of barium oxide and 8 parts of titanium dioxide aqueous solution into 5 parts of the mixed solution in the step (1), and carrying out ultrasonic treatment for 1 hour at the power of 300w to obtain a raw material solution; the barium compound in this example is barium oxide;
(3) drying the raw material liquid at 100 ℃ to constant weight, and calcining at 650 ℃ for 5 hours to prepare barium-containing catalyst powder;
(4) adding 3 parts of water to wet 10 parts of barium-containing catalyst powder, adding 2 parts of aluminum hydrosol, adding 2 parts of phenolic resin and 4 parts of ethanolamine, stirring to obtain a mixture, adjusting the water content of the mixture to 35%, and extruding the mixture into a honeycomb wet body by a double-screw extrusion method to obtain the barium-containing denitration catalyst; wherein the double screw extrusion method and the water content adjusting method are the prior art.
Example 4
The properties of the barium-containing catalysts obtained in examples 1 to 3 were measured by the prior art method
The barium-containing catalyst prepared in the embodiment 1-the embodiment 3 has the denitration efficiency of more than 95% in the temperature range of 300-400 ℃.
The axial and radial directions can reach 3.5MPa and 1.0MPa respectively.
The above examples are only intended to illustrate the technical solution of the present invention, but not to limit it; although the present invention has been described in detail with reference to the foregoing embodiments, it will be understood by those of ordinary skill in the art that: the technical solutions described in the foregoing embodiments may still be modified, or some technical features may be equivalently replaced; and such modifications or substitutions do not depart from the spirit and scope of the corresponding technical solutions of the embodiments of the present invention.
Claims (8)
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN114308008A (en) * | 2021-11-24 | 2022-04-12 | 安徽元琛环保科技股份有限公司 | Porous reduced TiO based on Ba doping2Preparation method of ultralow-temperature denitration catalyst |
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|---|---|---|---|---|
| CN114308008A (en) * | 2021-11-24 | 2022-04-12 | 安徽元琛环保科技股份有限公司 | Porous reduced TiO based on Ba doping2Preparation method of ultralow-temperature denitration catalyst |
| CN114308008B (en) * | 2021-11-24 | 2024-01-23 | 安徽元琛环保科技股份有限公司 | Porous reduction TiO based on Ba doping 2 Preparation method of ultra-low temperature denitration catalyst |
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